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Heterogeneous Fe3 single-cluster catalyst for ammonia synthesis via an associative mechanism

Author

Listed:
  • Jin-Cheng Liu

    (Tsinghua University)

  • Xue-Lu Ma

    (Tsinghua University)

  • Yong Li

    (Tsinghua University)

  • Yang-Gang Wang

    (Tsinghua University)

  • Hai Xiao

    (Tsinghua University)

  • Jun Li

    (Tsinghua University)

Abstract

The current industrial ammonia synthesis relies on Haber–Bosch process that is initiated by the dissociative mechanism, in which the adsorbed N2 dissociates directly, and thus is limited by Brønsted–Evans–Polanyi (BEP) relation. Here we propose a new strategy that an anchored Fe3 cluster on the θ-Al2O3(010) surface as a heterogeneous catalyst for ammonia synthesis from first-principles theoretical study and microkinetic analysis. We have studied the whole catalytic mechanism for conversion of N2 to NH3 on Fe3/θ-Al2O3(010), and find that an associative mechanism, in which the adsorbed N2 is first hydrogenated to NNH, dominates over the dissociative mechanism, which we attribute to the large spin polarization, low oxidation state of iron, and multi-step redox capability of Fe3 cluster. The associative mechanism liberates the turnover frequency (TOF) for ammonia production from the limitation due to the BEP relation, and the calculated TOF on Fe3/θ-Al2O3(010) is comparable to Ru B5 site.

Suggested Citation

  • Jin-Cheng Liu & Xue-Lu Ma & Yong Li & Yang-Gang Wang & Hai Xiao & Jun Li, 2018. "Heterogeneous Fe3 single-cluster catalyst for ammonia synthesis via an associative mechanism," Nature Communications, Nature, vol. 9(1), pages 1-9, December.
    • Handle: RePEc:nat:natcom:v:9:y:2018:i:1:d:10.1038_s41467-018-03795-8
    DOI: 10.1038/s41467-018-03795-8
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    Cited by:

    1. Tomohiro Tsuda & Min Sheng & Hiroya Ishikawa & Seiji Yamazoe & Jun Yamasaki & Motoaki Hirayama & Sho Yamaguchi & Tomoo Mizugaki & Takato Mitsudome, 2023. "Iron phosphide nanocrystals as an air-stable heterogeneous catalyst for liquid-phase nitrile hydrogenation," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
    2. Shuo Zhang & Jianghua Wu & Mengting Zheng & Xin Jin & Zihan Shen & Zhonghua Li & Yanjun Wang & Quan Wang & Xuebin Wang & Hui Wei & Jiangwei Zhang & Peng Wang & Shanqing Zhang & Liyan Yu & Lifeng Dong , 2023. "Fe/Cu diatomic catalysts for electrochemical nitrate reduction to ammonia," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    3. Xin Zhao & Fengliang Wang & Xiangpeng Kong & Ruiqi Fang & Yingwei Li, 2022. "Subnanometric Cu clusters on atomically Fe-doped MoO2 for furfural upgrading to aviation biofuels," Nature Communications, Nature, vol. 13(1), pages 1-9, December.
    4. Qian Wu & Chencheng Dai & Fanxu Meng & Yan Jiao & Zhichuan J. Xu, 2024. "Potential and electric double-layer effect in electrocatalytic urea synthesis," Nature Communications, Nature, vol. 15(1), pages 1-11, December.

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